A vertically aligned carbon nanotube (VACNT) array is a promising candidate for a high-performance thermal interface material in high-power microprocessors due to its excellent thermal transport property. However, its rough and entangled free tips always cause poor interfacial contact, which results in serious contact resistance dominating the total thermal resistance. Here, we employed a thin carbon cover to restrain the disorderly growth of the free tips of a VACNT array. As a result, all the free tips are seamlessly connected by this thin carbon cover and the top surface of the array is smoothed. This unique structure guarantees the participation of all the carbon nanotubes in the array in the heat transport. Consequently the VACNT array grown on a Cu substrate shows a record low thermal resistance of 0.8 mm(2) K W-1 including the two-sided contact resistances, which is 4 times lower than the best result previously reported. Remarkably, the VACNT array can be easily peeled away from the Cu substrate and act as a thermal pad with excellent flexibility, adhesive ability and heat transport capability. As a result the CNT array with a thin carbon cover shows great potential for use as a high-performance flexible thermal interface material.